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HyET Hydrogen, a Dutch developer of hydrogen compression and purification equipment, and the National Renewable Energy Laboratory (NREL) are collaborating to develop membrane electrode assembly (MEA) manufacturing automation technology for electrochemical hydrogen compression (EHC). EHC has the potential to outcompete mechanical compression for hydrogen end-use applications.
The Molten Salt Reactor Experiment (MSRE) was a prototype nuclear reactor which operated from 1965 to 1969 at Oak Ridge National Laboratory. The MSRE used liquid fluoride salts as a heat transfer fluid and solvent for fluoride based {sup 235}U and {sup 233}U fuel. Extensive research was performed in order to optimize the removal of oxide and metal impurities from the reactor's heat transfer salt, 2LiF-BeF{sub 2} (FLiBe). This was done by sparging a mixture of anhydrous hydrofluoric acid and hydrogen gas through the FLiBe at elevated temperatures. The hydrofluoric acid reacted with oxides and hydroxides, fluorinating them while simultaneously releasing water vapor. Metal impurities such as iron and chromium were reduced by hydrogen gas and filtered out of the salt. By removing these impurities, the corrosion of reactor components was minimized. The Univ. of Wisconsin - Madison is currently researching a new chemical purification process for fluoride salts that make use of a less dangerous cleaning gas, nitrogen trifluoride. Nitrogen trifluoride has been predicted as a superior fluorinating agent for fluoride salts. These purified salts will subsequently be used for static and loop corrosion tests on a variety of reactor materials to ensure materials compatibility for the new FHR designs. Demonstration of chemistry control methodologies along with potential reduction in corrosion is essential for the use of a fluoride salts in a next generator nuclear reactor system. (authors)
The National Nuclear Laboratory (NNL) treats a wide variety of materials produced as by-products of the nuclear fuel cycle, mostly from uranium purification and fuel manufacture but also including materials from uranium enrichment and from the decommissioning of obsolete plants. In the context of this paper, treatment is defined as recovery of uranium or other activity from residues, the recycle of uranium to the fuel cycle or preparation for long term storage and the final disposal or discharge to the environment of the remainder of the material. NNL's systematic but flexible approach to residue assessment and treatment is described in this paper. The approach typically comprises up to five main phases. The benefits of a systematic approach to waste and residue assessments and processing are described in this paper with examples used to illustrate each phase of work. Benefits include early identification of processing routes or processing issues and the avoidance of investment in inappropriate and costly plant or processes. (authors)
Recovery of Cs-137 from HLW and its utilisation as source pencil in place of Co-60 is vital for medical and sewage treatment applications in India. For separation of Cs, specific ion exchange resins as well as 'Calyx crown' solvent have been developed and synthesized indigenously. A flow sheet involving separation of Cs from acidic HLW using Ammonium Molybdo Phosphate (AMP) resins, recovery of Cs from the loaded AMP column by dissolving it in alkali, ion exchange purification of Cs rich alkaline solution using Resorcinol-Formaldehyde Poly condensate (RF) resins and its elution in cesium nitrate form was developed and demonstrated. Solvent extraction route employing 0.03 Molar, 1-3-octyl oxy Calyx (4) arene crown-6 in 30% isodecyl alcohol and dodecane was also established using mixer settlers. Cesium lithium borosilicate glass based formulations have been considered as a glass matrix for Cs irradiation pencils. While choosing this vitreous matrix, attributes addressing maximum possible Cs-137 loading, low glass pouring temperature to minimise Cs volatility, reasonably good mechanical strength and good chemical durability have been considered. Recovered cesium nitrate solution was vitrified along with glass additives in an induction heated metallic melter and subsequently poured into 12 numbers of Cs irradiation pencils positioned on turn-table equipped with the load cell. The complete cycle involving recovery of Cs from HLW followed by its conversion into Cs pencil was demonstrated. (authors)
The Department of Energy (DOE) is working to de-inventory sites and consolidate hazardous materials for processing and disposal. The DOE administers a wide range of certified shipping packages for the transport of hazardous materials to include Special Nuclear Material (SNM), radioactive materials, sealed sources and radioactive wastes. A critical element to successful and safe transportation of these materials is the availability of certified shipping packages. There are over seven thousand certified packagings (i.e., Type B/Type AF) utilized within the DOE for current missions. The synergistic effects of consolidated maintenance, refurbishment, testing, certification, and costing of these services would allow for efficient management of the packagings inventory and to support anticipated future in-commerce shipping needs. The Savannah River Site (SRS) receives and ships radioactive materials (including SNM) and waste on a regular basis for critical missions such as consolidated storage, stabilization, purification, or disposition using H-Canyon and HB-Line. The Savannah River National Laboratory (SRNL) has the technical capability and equipment for all aspects of packaging management. SRS has the only active material processing facility in the DOE complex and is one of the sites of choice for nuclear material consolidation. SRS is a logical location to perform maintenance and periodic testing of the DOE fleet of certified packagings. This initiative envisions a DOE Eastern Packaging Staging and Maintenance Center (PSMC) at the SRS and a western hub at the Nevada National Security Site (NNSS), an active DOE Regional Disposal Site. The PSMC's would be the first place DOE would go to meet their radioactive packaging needs and the primary locations projects would go to disposition excess packaging for beneficial reuse. These two hubs would provide the centralized management of a packaging fleet rather than the current approach to design, procure, maintain and dispose of packagings on a project-by-project basis. This initiative provides significant savings in packaging costs and acceleration of project schedules. In addition to certified packaging, the PSMC would be well suited for select designs of 7A Type A packaging and Industrial Packaging. (authors)
Co-processing process, which is the modified Purex process focused on co-recovery of Pu and U, has been studied at Operation Testing Laboratory, Tokai Reprocessing Plant in JAEA. The set up of the process was performed with flow-sheets study by process calculation to avoid Pu isolation in the whole process and to co-recover Pu/U product solution with a suitable Pu/U ratio (0.5< Pu/U <2). The initial Pu/U ratios of the feed solutions were taken as 1%, 3% and 20% considering the composition of the future spent fuels. The verification of the flow-sheets for each feed solutions were carried out with mixer-setters and active Pu/U feed solutions, focusing on the partitioning unit, and favorable back extraction performances of Pu accompanied by U were observed at all cases of the given feed solutions. According to these results, the co-processing process showed a good prospect to treat all kinds of future fuels from LWR, LWR-MOX and FBR, and a good prospect to be simplified by omitting the Pu/U purification cycle.
A study is under progress to examine the feasibility of single stream Molten Salt Actinide Recycling and Transmuting system without and with Th support (MOSART) fuelled with different compositions of actinide tri-fluorides (AnF{sub 3}) from used LWR fuel. New fast-spectrum design options with homogeneous core and fuel salts with high enough solubility for AnF{sub 3} are being examined because of new goals. The flexibility of single fluid MOSART concept with Th support is underlined, particularly, possibility of its operation in self-sustainable mode (Conversion Ratio: CR=1) using different loadings and make up. The paper summarizes the most current status of fuel salt and container material data for the MOSART concept received within ISTC-3749 and ROSATOM-MARS projects. Key physical and chemical properties of various fluoride fuel salts are reported. The issues like salt purification, the electroreduction of U(IV) to U(III) in LiF-ThF{sub 4} and the electroreduction of Yb(III) to Yb(II) in LiF-NaF are detailed.
This paper analyzes absorption spectra of molten salts containing some of the actinide and rare-earth elements (REE) and evaluated the prospects of using the individual transitions to control the composition of the spent molten salts using adsorption and luminescence spectroscopy from the standpoint of the theory of Judd-Ofelt. It is shown that the fluorescent method can be recommended only for the monitoring of the degree of purification of the molten salt from the REE in the final stage, when only trace amounts of fission products are in the molten salt. In this case, the content of REE in the molten process is much smaller than that of the used model samples and that eliminates the problem of a significant decrease in the population levels of fluorescent Eu{sup 3+} by quenching impurities. In addition, the presence of salt in the matrix of americium and curium can cause self-luminescence of Eu{sup 3+} due to alpha disintegration energy of transuranics, which also complicates the quantitative measurement of luminescence for the determination of REE.
The modeling approach for process design is illustrated in this paper by the work done to qualify the PAREX code to design the flow sheet of a uranium/plutonium splitting operation in a pulsed column. The different flow sheet experimentations are presented along with the simulation results. The qualified code has been successfully used to design the flow sheet of this operation in the first purification cycle of UP2-800 plant at La Hague. (authors)
Organic ion exchangers (IEX) play a major and increasing role in the reactor coolant and other water purification processes. During their operation time they receive significant amounts of radioactivity, making their disposal, together with their organic nature, as medium active waste challenging. Processes applied so far do not eliminate the organic matter, which is unwanted in disposal facilities, or, if high temperatures are applied, raise problems with volatile radionuclides. NUKEM Technologies offers their well introduces process for the destruction of spent solvent (TBP), the pebble bed pyrolysis, now for the treatment of spent IEX (and other problematic waste), with the following benefits: the pyrolysis product is free of organic matter, and the operation temperature with approx. 500 deg. C keeps Cs radionuclides completely in the solid residue. (authors)
Ion-exchange resins are used in the purification of coolant water in boiling water reactor nuclear power plants. The spent resins are a form of low-level or intermediate-level radioactive waste. These resins may have a relatively high specific activity level and are normally transported to a disposal facility within a secondary container placed in a Type B transportation cask. During transportation, hydrogen gas may build up in the cask due to radiolysis of the hydrogenous material in the contents. In the licensing process, a Type B cask is carefully analyzed to ensure that the maximum amount of hydrogen gas generated does not exceed 5%. The calculation to determine the mole fraction of hydrogen gas generated is a function of many variables, including the properties of the contents and the volume ratios of the contents. Because water generates hydrogen gas when it undergoes radiolysis, the amount of water present in the waste is normally limited. Typically, Type B transportation casks are allowed to carry dewatered resins, meaning less than 1% free-standing water by volume. To ensure compliance with this limitation, the dewatering process requires specialized equipment to pump the water from the secondary container. In an effort to enhance the usability of the RT-100 Type B transportation cask, Robatel Technologies re-analyzed the hydrogen gas generation calculation for contents including 'grossly dewatered' resins. Grossly dewatered resins are defined as resins containing less than 20% free-standing water by volume. This higher limit is made possible by a more thorough hydrogen gas generation calculation, which ensures that the flammability limit is not reached during shipment. In July 2015, The USNRC issued Revision 1 of the Certificate of Compliance for the Robatel Technologies RT-100 Type B transportation cask. This revision allows the cask to be used for grossly dewatered resins. With the revised Certificate of Compliance, the RT-100 is the first of its kind whose authorized contents include greater than 1% free liquids by volume. As a result of this change, the cask user can meet the 20% maximum free-standing water volume with a much simpler gravity-driven dewatering process. It is no longer necessary to have a complex dewatering system to ensure compliance with regulatory requirements. (authors)
WOW presents its revolutionary technology and equipment for liquid radioactive waste treatment: outperforming ultimate water decontamination and purification process, enhanced sludge concentration, no secondary waste nor consumables, fully automated, remote controlled and self-decontaminating device. The WOW's technology is based upon a never before observed discovery of fluid dynamics science: the possibility of performing a molecular separation between solute and suspended elements and the solvent. The combination of such a molecular separation process with a standard vacuum evaporation improves the abatement performances by thousands of times, with respect to those of the state of the art vacuum evaporators. In addition to this, no secondary waste is produced during the process, as no filters, membranes, resins or additives are used. WOW equipment, automated and remote controlled, self decontaminates after use and can be designed and constructed either tailored to the application needs or with a modular approach for enhanced transportability and application flexibility. After the preliminary verification by CNR, the Italian National Research Center, WOW Technology's decontamination device was tested c/o LENA, the Laboratory of Applied Nuclear Energy of the University of Pavia, Italy with a simulated solution 6000 times more contaminated than the nuclear reactor's cooling water of Fukushima-Daiichi NPP. In addition to that, WOW's technology was also used in a real case at the Radiochemistry laboratory of the Pavia's University Chemistry department. Both the above mentioned contaminated fluids have been successfully decontaminated without production of additional or secondary waste. WOW's technology has already performed on industrial scale c/o the Nuclear Repository of S.S.M. in Saluggia, Italy: 45000 liters of acid radioactive solution have been successfully decontaminated to a Decontamination Factor (DF) of 335000 for Cs-137 by one single evaporation step and without using any additional tool to control steam. [Performances independently certified by: National Physics Laboratory (UK) and Pavia University Radiochemistry Laboratory, Chemistry Department (Italy)]. The high decontamination factors and the high volume reduction of the sludge make this technology suitable for the ultimate treatment of highly contaminated liquid waste such as the Fukushima-Daiichi nuclear reactor's cooling water. The WOW's technology addresses as well to interventions in both, operating and decommissioning nuclear power plants and any other nuclear and radioactive facility whose produced and/or stored radioactive liquid solutions, including acid liquid solutions, can be successfully treated, the waste volume reduced and no secondary waste produced. (authors)
The filter cartridges used in water purification system of the IEA-R1 research reactor become radioactive waste after the end of their useful life. The characterization of this waste is one step in their management, which aims at identifying and quantifying the radionuclides present, including those known as 'difficult to measure' (DTM) radionuclides. Wastes from nuclear reactors contain fission and activation products and transuranic elements, only few of them emitting gamma radiation measurable by simple gamma spectrometry methods. In routine waste management activities, the concentrations of the DTM can only be estimated by indirect methods such as scaling factors. The method of the scaling factors uses empirically determined proportions between the concentrations of DTM radionuclides and that of easily measurable gamma emitters called key nuclides (KN), to calculate DTM concentrations. Determining the scaling factors for the filter cartridges is a hard task when the number of samples is large, not only because the preparation of samples is difficult but also because the number of radionuclides to analyze is large. If it can be demonstrated that DTM and KN are both distributed evenly in the filters, less samples from each filter are necessary, reducing lab work. The aim of this paper is to present the results of the assessment of homogeneity along the filter cartridges by gamma spectrometry of chemically reduced samples. Five thin slices of five filters were burnt and the ashes quantitatively dissolved and the activity concentration of the solutions determined by gamma spectrometry. (authors)
The recent natural gas drilling boom has brought heightened attention to the issue of TENORM waste management. Radioactive residues from the extraction, treatment, and purification of materials containing uranium and thorium, or their progeny, pose a public health hazard primarily in the form of ground water contamination. Hydraulic fracturing can liberate formation waters from shale; the high salinity of which can cause radium to move with the water to the surface. The disposal and handling of this water has been a subject of public controversy. For soil remediation projects, radium-226 is generally one of the radionuclides of concern due to its alpha emissions. However performing a survey scan for Ra-226 is difficult because its photon emissions are low energy and have minimal probability of emission per decay (186.2 keV, 3.3% abundance). Additionally resolving its emission from U-235 (185.7 keV, 57% abundance) with field instrumentation is not feasible. Therefore detection of Ra-226 relies on the presence and photon emissions of its progeny. This paper outlines methodology for calculating the minimum detectable concentration of Ra-226 in characterization scans using a sodium-iodide detector array coupled with a multi-channel analyzer. Using progeny ingrowth as a detection proxy requires knowing decay time in order to determine progeny emission rates. Knowledge of site history, process, and prior survey results can be key in determining an accurate decay time. However in the absence of such information in-situ measurements can be used to estimate decay time by comparing observed progeny emission ratios against established values. These values are determined using Oak Ridge National Laboratory's ORIGEN-ARP program to generate photon energy spectra for Ra-226 and its progeny at specified time intervals. Once decay time is established, the detector's minimum detectable concentration can be calculated by synthesizing the expected emission spectra and Los Alamos National Laboratory's Monte Carlo N-Particle transport code to simulate detector response. Traditionally, one of the steps in calculating a system's minimum detectable concentration is to place an appropriate button source under the detector, record the response, and then move the source by a specified increment. This process is repeated until the detector's spatial efficiency has been mapped. Due to the impracticality of performing this with Ra-226 button sources of varying decay times, Monte Carlo N-Particle transport code was utilized to determine the detector's spatial efficiency. A dime sized source with the established emission spectra was placed into the center of a rectangle of soil. This rectangle, including the source, was used as a lattice element to fill the region of space below the detector. The simulation was designed to track the energy distribution of pulses created in the sodium iodide crystal using the F8 tally, and was setup to isolate each source; thereby correlating detector response to source position. The simulation output required post-processing to determine conversion factors from counts per second to disintegrations per second. Post-processing accounted for subtraction of the Compton continuum, and average the data over the scanning pattern to obtain the expected spatial sensitivity during a characterization study. This was performed for the following photo-peaks: 609 keV (Bi-214), and 1764 keV (Bi-214). For calculation of the scan minimum detectable concentration, the surveyor efficiency coefficient from NUREG 1507 was supplanted in favor of a scan speed deviation factor. This was used because the detector utilizes computerized data collection (spatial and spectral). This report finds that, for two shielded 10.16 cm x 10.16 cm x 40.64 cm sodium-iodide crystals with integrated multi-channel analyzers, the minimum detectable concentration in surface soils is less than 1 pCi per gram Ra-226 for a 1 second survey measurement. These results assume a volumetric source with a maximum depth of 15.24 cm and a minimum decay time of 21 days. Verification of the system's capabilities was performed by sending soil samples from scanned areas, and locations where in-situ measurements were performed, to an independent laboratory for analysis. The laboratory results demonstrated that scanned area was principally comprised of soil containing less than 1 pCi per gram Ra-226. This borders the system MDC and it underestimated the concentration of radium in the soil. The probable causes of this is escape of radon gas from the surface soil. Radon is the daughter of radium, and has a high mobility in soil. If the gas escapes, then the progeny used as the detection proxy will be present in lower than expected concentrations. Radionuclide identification using high volume sodium-iodide crystals in low level characterization scans is demonstrated to be possible. Further system refinement will focus on developing a methodology to estimate a radon escape factor for site specific use. Accounting for radon escape in the top 15.24 cm of soil will allow the system to better estimate Ra-226 concentrations in soil. This is a significant advancement over the gross counting statistics used in most studies to satisfy MARSSIM survey requirements, because it will increase stakeholder confidence. (authors)
The Daher-TLI UF{sub 6} Cylinder Service Center (UCSC) began operation in 2013 and functions as a dedicated wash, re-certification, storage and disposal facility for 122 cm uranium hexafluoride (UF{sub 6}) cylinders. The primary purpose of the facility is to provide cylinder cleaning and re--certification services to the UF{sub 6} industry for cylinders that previously contained natural or depleted UF6. The facility also has the ability to recover most of the uranium in the form of uranyl peroxide (UO{sub 4}) or triuranium octoxide (U{sub 3}O{sub 8}). Small residues of UF{sub 6} (commonly referred to as a heel) from natural cylinders are removed and treated in a patented three-step purification process that recovers U{sub 3}O{sub 8} that meets the ASTM specification. The wastewater ordinarily contains a mixture of sodium salts (77% sodium sulfate, 23% sodium nitrate) along with minute traces of uranium (1 - 2 mg/L) and fluoride (10 - 20 mg/L). Over a period of 6 months, lab analyses were performed on the filtrate from a legacy cylinder in an attempt to separate uranium and fluoride from this stream. These pilot results established near quantitative recovery of uranium (< 1 mg/L) and near complete separation of fluorides (5 - 15 mg/L). This paper follows the efforts of the Daher-TLI UCSC to process the abnormal heeled UF{sub 6} cylinder. This paper also documents the lessons learned from this experience and how those lessons were used to improve the UCSC wash process. These modifications served to recover 99.87% of the input uranium as UO{sub 4} while simultaneously creating a waste stream with only trace amounts of impurities. (authors)
On May 2012, Best Medical Belgium S.A. (BMB), a manufacturer of pharmaceutical products located on the nuclear site of Fleurus, was declared bankrupt. According to the Belgian law, ONDRAF/NIRAS (Belgian Radioactive Waste Management Agency) was entrusted with the clean-up and decommissioning operations of the former BMB facilities, nowadays known as 'ONDRAF Site Fleurus' (ONSF). In June 2015, ONSF launched a Decontamination and Decommissioning (D and D) program, for which Tractebel: - Supports the definition of the clean-up and decommissioning strategies; - Drafts the Final Decommissioning Plan (FDP) and Safety Analysis Report (SAR) that will be submitted to FANC/AFCN (Belgian Federal Agency for Nuclear Control) in order to get the License for decommissioning; - Drafts the technical specifications of the public tendering process related to the D and D program; - Ensures the day to-day follow-up of the D and D activities on site. Four nuclear buildings are part of the D and D activities. One of them, building 14 (B14), represents the most challenging and extensive task with the clean-up of highly contaminated areas and its further decommissioning up to the final state. This building features two cyclotrons (CGR and IBA cyclotrons) successively used to produce radioisotopes, as well as hot cells and glove boxes used for their purification and the conditioning of the final pharmaceutical product. The present paper aims at presenting the most recent development steps of the clean-up phase regarding the adaptations of existing facilities and the upcoming activities in preparation of the decommissioning activities. To allow the sorting and the treatment of the radioactive material identified in the physical and radiological inventory, several workshops have been implemented within the B14 building in order to deal with radioactive materials arising from the clean-up and D and D activities. Following the conceptual design phase, Tractebel has actively monitored the on-site activities for the construction of those workshops such as: - The modification of the civil works; - The revamping of the ventilation system; - The installation of dedicated lifting equipment and workstations equipped with cutting devices; - The assembly of a docking station for filling the radioactive packages. The removal of the activated concrete surrounding the IBA cyclotron requires the erection of a containment structure and an extension structure. The containment structure, composed of light metallic beams, is located above the cyclotron and its irradiation zones. For operational security reasons and working efficiency, the cutting process of the concrete ceilings and walls will be performed from the top inside the containment structure by means of an eight tons overhead bridge crane. Concrete blocks resulting from the cutting process will then be lifted, without any loss of containment, towards the extension zone of the nuclear zone of the IBA cyclotron for further resizing, sorting and evacuation towards the identified waste routes. To prepare this task which will be performed during the decommissioning phase, Tractebel sets up the necessary technical specifications. (authors)
The High Flux Reactor (HFR) in Petten (NL) has been producing medical isotopes for several decades. Additionally, the HFR is used for many experiments including fuel/material tests. Over the years, Ion Exchange Resins (IER) that are used for the purification of the primary circuit and the basin have been replaced. Spent IER were accumulated and stored on site. Over time, the IER has become a historical waste issue that needs to be solved pragmatically as space to store them on site becomes scarce. This paper provides an overview of the characterization methodology needed to manage the Ion Exchange Resin wastes. (authors)
A molten salt phase is used as the solvent in pyrochemical reprocessing. The molten salt waste generated in pyro-processes contains the residual lanthanides and actinides as various compounds. Various methods have been proposed for recovering and recycling these useful elements. The separation of actinides from lanthanides is performed by electrolysis or reductive extraction. Herein we have studied PyroRedSox-based co-reduction of Nd and Bi via electrolysis in a molten chloride salt. The redox behavior of Nd and the formation potential of intermetallic compounds of Nd and Bi were determined using cyclic voltammetry (CV). Electrorefining was performed under a constant reductive potential at 773 K in LiCl-KCl eutectic mixture; the co-reduction potential was -1.37 V. Lastly, the co-reduction potential of the intermetallic compound was applied to reduce the amount of Nd and Bi. Scanning electron microscopy (SEM) revealed that various kinds of intermetallic compounds were formed in Bi and Nd, and were deposed in the lower part of the molten salt, allowing purification of the contaminated molten salt. (authors)